The DFT labeled dataset of hydrated Ni-Al LDH structures and bulk-solution, interfacial, and confined configurations containing NaCl, NaBr, NaNO3 or Na2SO4.

The reference energies, atomic forces and analytical stress tensors were calculated with CP2K under three-dimensional periodic boundary conditions with the gamma point sampling. The revPBE exchange-correlation functional was combined with the D3(BJ) dispersion correction. DZVP-MOLOPT-SR-GTH basis sets and GTH-PBE pseudopotentials were used, with plane-wave density and relative cutoffs of 500 and 50 Ry, respectively. The inner and outer SCF convergence thresholds were both set to 10-6. A geometry-deduplicated dataset of 4,755 DFT-labeled configurations was assembled from Dual-space Chemical-Bond-level Fine (DCBF) sampling method. The dataset cover hydrated Ni-Al LDH structures and bulk-solution, interfacial, and confined configurations containing NaCl, NaBr, NaNO3 or Na2SO4.